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Transformational Membranes for
Pre-combustion Carbon Capture
DE-FE0031635
Winston Ho / Yang HanWilliam G. Lowrie Department of Chemical & Biomolecular Engineering
Department of Materials Science and Engineering
The Ohio State University
2019 NETL Technologies Integrated Review Meeting
Pittsburgh, PA, August 27, 20191
Project Objective
• Develop a cost-effective design and fabrication process for a novel transformational membrane and its membrane modules that capture CO2 from coal-derived syngas
• 95% CO2 Purity
• >99% H2 Recovery
• COE 30% Less than Baseline Approaches
2
2-Budget Period Project
• BP1: 10/01/2018 – 03/31/2020– Laboratory-scale membrane synthesis, characterization and
transport performance studies– High-level preliminary techno-economic analysis
• BP2: 04/01/2020 – 09/30/2021– Laboratory-scale membrane synthesis, characterization and
transport performance studies to continue– Fabrication, characterization and transport performance
studies of scale-up membrane (14″ wide by 20′ long) – Fabrication, performance and stability testing of spiral-wound
membrane modules– Update techno-economic analysis performed in BP 1
3
• Integrated program with fundamental studies, applied research, synthesis, characterization and transport studies, and high-level techno-economic analysis
4
Funding and Performance Dates
• Total Budget: 10/01/2018 – 09/30/2021 DOE: $799,988; OSU: $199,998 (20% cost share)
• BP1: 10/01/2018 – 03/31/2020 DOE: $386,694; OSU: $96,674
• BP2: 04/01/2020 – 09/30/2021 DOE: $413,294; OSU: $103,324
5
Technical Background: Proposed Process
•Proposed membrane process does not require significant syngas cooling (compared to competition)
31.7 bar
54.1 bar, 31% CO2
50 bar 153 bar
>95% CO2
31.7 bar
4% CO2
<10 ppm H2S
H2S
Removal
(Selexol)
6
Location of Proposed Technology in
IGCC Plant
Selective Amine Polymer Layer / Polymer Support
Simplicity of Membrane for Low Cost
7
≈ ≈
≈
Selective amine polymer layer
(~15 µm, dense layer)
Nonwoven fabric backing
(~100 μm)
Polymer support(~20 μm, Ø ~10 nm)
8
Amine Polymer Layer Contains Mobile and Fixed Carriers: Facilitated Transport
CO2 CO2
Membrane
CO2+
CO2
CO2
CO2
Mobile
Carrier
Facilitated Transport
Feed Side Permeate Side
Non-Reacting
Gas: H2H2
Physical Solution-Diffusion
Mobile
Carrier
CO2
Mobile
Carrier
CO2
Mobile
Carrier
9
Tunable Amine-CO2 Chemistry
• Reaction of CO2 with Unhindered Amines
CO2 + R–NH2 ⇌ R–NH2+–COO–
R–NH2+–COO– + R–NH2 ⇌ R–NH–COO– + R–NH3
+
Overall:
CO2 + 2 R–NH2 ⇌ R–NH–COO– + R–NH3+
• Reaction of CO2 with Hindered Amines
CO2 + R1–NH–R2 ⇌ R1R2–NH+–COO–
R1R2–NH+–COO– + H2O ⇌ R1R2–NH2+ + HCO3
-
Overall: Can double the CO2 capacity
CO2 + R1–NH–R2 + H2O ⇌ R1R2–NH2+ + HCO3
-
Facilitated Transport vs.Solution-Diffusion Mechanism
• CO2 Facilitated Transport Flux: Very High– CO2-amine reaction enhances CO2 flux
• H2 Flux: Very Low– H2 does not react with amine
– H2 transport follows conventional physical solution-
diffusion mechanism, which is very slow
10
10
100
1000
180 200 220 240 260 280 300 320
CO
2/H
2s
ele
cti
vit
y
CO2 permeance (GPU)11
Membrane Performances
BP1Q1
BP1Q2
BP1Q3
Enhanced
Physical
Solubility
Enhanced
Chemical
Solubility
12
Membrane Performances
Simulated Syngas at 107°C and 31.7 bar
Effect of Carrier Saturation Phenomenon on Performance
13
Effect of CO2 Permeance on Cost of Electricity Increase
0
5
10
15
20
25
30
35
14
15
16
17
18
19
50 100 150 200 250 300 350 400 450 500
Mem
bra
ne a
rea (
×10
4m
2)
CO
E in
cre
ase (
%)
CO2 permeance (GPU)
COE increase
Membrane area
COE increase
of BP1Q1COE increase
of BP1Q2
COE increase
of BP1Q3
14
Membranes Synthesized with Tuned H2S/CO2 Selectivities
0
3
6
9
0 1 2 3 4 5 6 7 8 9 10 11 12 13
H2S
/CO
2s
ele
cti
vit
y
Feed CO2 partial pressure (bar)
Membrane M6
Membrane BP1Q3
15
Effect of H2S/CO2 Selectivity on H2S Concentration in H2 Product
16
0.1
1
10
100
1000
10000
1 2 3 4 5 6
Sw
eet
syn
gas H
2S
(p
pm
v)
H2S/CO2 selectivity
< 6 ppm H2S
for BP1Q3
Plans for Future Testing/Development
17
• Remaining BP1– Increase CO2 Sorption at High Pressure
– Enhance Membrane Mechanical Properties
– Preliminary Techno-Economic Analysis
• BP2– Membrane Scale-up and Characterization
+ Continuous roll-to-roll fabrication (14″ wide by 20′ long)
– Prototype SW Module Fabrication
+ Fabricate 9 prototype SW modules (800 cm2 each)
+ 200-h stability test with simulated syngas
– Final Techno-Economic Analysis
18
Acknowledgments
David Lang & José Figueroa, DOE/NETL
Financial Support
DOE/NETLDE-FE0031635
– Federal funding for membrane development
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